Catalisadores a base de Pt suportados em matrizes mesoporosas de carbono visando a reação de eletrooxidação de glicerol
Autor(a) principal: | |
---|---|
Data de Publicação: | 2018 |
Tipo de documento: | Dissertação |
Idioma: | por |
Título da fonte: | Repositório Institucional da UFSCAR |
Texto Completo: | https://repositorio.ufscar.br/handle/ufscar/10907 |
Resumo: | This work aimed the synthesis, characterization and electrochemical tests of Pt and Pt-Sb nanoparticle catalysts onto mesoporous carbon applied to glycerol electrooxidation reaction. Specifically, the carbon matrixes were synthetized from Si templates with distinct geometries, giving CMK-3 and CMK-5 3D structures. These structures were treated in O2-free atmospheres at 1173 K for 5 h and after the removal of Si with HF solution (as confirmed by thermogravimetric analysis), the mesoporous structures were attested by Small Angle X-Ray diffraction and a 4.8 and 5.3 nm porous diameters were estimated by nitrogen adsorption isotherms to the CMK-3 and CMK-5 structures, respectively. Pt nanoparticles synthesis onto carbon structures (Pt/C) were performed by direct reduction of chloroplatinic acid (H2PtCl6) with formic acid giving particles with 4.5 nm mean diameters as reveled by transmission electron microscopy. Finally, Pt-Sb/C catalysts were produced by irreversible Sb2O3 adsorption. Pt/C catalysts showed voltammetric profiles consistent with metallic Pt in 0.5 mol L-1 H2SO4 solutions, certifying the synthesis success. In the presence of glycerol, it was observed that the activity to the oxidation happens at potential higher than 0.8 V regardless the carbon support; on the other hand, Pt-Sb/C shifted the reaction onset in ca -0.3 V and maintained this activity under fixed potential (0.5 V). Pt-Sb/CMK-3 depicted the best activity among the synthetized catalysts, providing currents 1.6 and 2.0 times bigger than those in Pt-Sb/CMK-5 and Pt-Sb/Vulcan, respectively. |
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Andrade, Renato Nunes deSitta, Elton Fabianohttp://lattes.cnpq.br/4326476348284298http://lattes.cnpq.br/9933821460129238d16278b3-dc1e-43a7-a061-b1e1c2c029592019-02-05T13:24:59Z2019-02-05T13:24:59Z2018-08-24ANDRADE, Renato Nunes de. Catalisadores a base de Pt suportados em matrizes mesoporosas de carbono visando a reação de eletrooxidação de glicerol. 2018. Dissertação (Mestrado em Química) – Universidade Federal de São Carlos, São Carlos, 2018. Disponível em: https://repositorio.ufscar.br/handle/ufscar/10907.https://repositorio.ufscar.br/handle/ufscar/10907This work aimed the synthesis, characterization and electrochemical tests of Pt and Pt-Sb nanoparticle catalysts onto mesoporous carbon applied to glycerol electrooxidation reaction. Specifically, the carbon matrixes were synthetized from Si templates with distinct geometries, giving CMK-3 and CMK-5 3D structures. These structures were treated in O2-free atmospheres at 1173 K for 5 h and after the removal of Si with HF solution (as confirmed by thermogravimetric analysis), the mesoporous structures were attested by Small Angle X-Ray diffraction and a 4.8 and 5.3 nm porous diameters were estimated by nitrogen adsorption isotherms to the CMK-3 and CMK-5 structures, respectively. Pt nanoparticles synthesis onto carbon structures (Pt/C) were performed by direct reduction of chloroplatinic acid (H2PtCl6) with formic acid giving particles with 4.5 nm mean diameters as reveled by transmission electron microscopy. Finally, Pt-Sb/C catalysts were produced by irreversible Sb2O3 adsorption. Pt/C catalysts showed voltammetric profiles consistent with metallic Pt in 0.5 mol L-1 H2SO4 solutions, certifying the synthesis success. In the presence of glycerol, it was observed that the activity to the oxidation happens at potential higher than 0.8 V regardless the carbon support; on the other hand, Pt-Sb/C shifted the reaction onset in ca -0.3 V and maintained this activity under fixed potential (0.5 V). Pt-Sb/CMK-3 depicted the best activity among the synthetized catalysts, providing currents 1.6 and 2.0 times bigger than those in Pt-Sb/CMK-5 and Pt-Sb/Vulcan, respectively.Esse trabalho teve como objetivos a síntese, caracterização e testes de catalisadores nanoparticulados de Pt e Pt-Sb em distintas matrizes mesoporosas de carbono, visando a catálise da reação de eletrooxidação glicerol. Especificamente, as matrizes de carbono foram sintetizadas em bases de Si com distintas geometrias, gerando estruturas 3D de carbono do tipo CMK-3 e CMK-5, que foram tratadas a 1173 K por 5 h em atmosfera isenta de oxigênio. Após a remoção do Si com solução de HF, confirmado por análises termogravimétrias, as estruturas mesoporosas foram atestadas por difração de raios-X a baixo ângulo e o tamanho dos poros (4,9 e 5,3 nm para CMK-3 e CMK-5, respectivamente) estimados por isotermas de fisissorção de nitrogênio. A formação das nanopartículas de Pt nas estruturas de carbono (Pt/C) foi realizada por redução direta de ácido hexacloroplatínico (H2PtCl6) com ácido fórmico. Análises de microscopia de transmissão eletrônica revelaram partículas com tamanho médio de 4,5 nm e com boa dispersão sobre os suportes. A formação de Pt-Sb/C foi realizada por adsorção irreversível de Sb2O3 aos catalisadores de Pt. Os catalisadores Pt/C mostraram perfis voltamétricos condizentes à Pt metálica em H2SO4 0,5 mol L-1 atestando que a síntese foi bem-sucedida. Na presença de glicerol, observou-se que, independentemente do tipo de suporte, a eletrooxidação de glicerol ocorre em potenciais superiores a 0,8 V vs. ERH, porém os catalisadores de Pt-Sb/C deslocaram o início da reação em ca – 0,3 V vs. ERH e mantiveram a taxa de reação em potencial fixo (0,5 V vs. ERH). A Pt-Sb/CMK-3 mostrou o melhor desempenho para a eletrooxidação de glicerol, apresentando valores de corrente de 1,6 e 2,0 vezes maiores que os obtidos com Pt-Sb/CMK-5 e Pt-Sb/Vulcan, respectivamente.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)porUniversidade Federal de São CarlosCâmpus São CarlosPrograma de Pós-Graduação em Química - PPGQUFSCarCélulas a combustíveisEletrocatáliseGlicerolFuel cellsElectrocatalysisGlycerolCMK3CMK5CIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICACatalisadores a base de Pt suportados em matrizes mesoporosas de carbono visando a reação de eletrooxidação de glicerolPt-based catalysts supported in mesoporous carbon matrix for glycerol electro-oxidation reactioninfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisOnline6006007b79dc94-df30-4f61-b9d4-558e9f522384info:eu-repo/semantics/openAccessreponame:Repositório Institucional da UFSCARinstname:Universidade Federal de São Carlos (UFSCAR)instacron:UFSCARORIGINALDissertacao - Renato Nunes de Andrade - PPGQ - UFSCar - 2018 - 2 .pdfDissertacao - Renato Nunes de Andrade - PPGQ - UFSCar - 2018 - 2 .pdfapplication/pdf3086710https://repositorio.ufscar.br/bitstream/ufscar/10907/1/Dissertacao%20-%20Renato%20Nunes%20de%20Andrade%20-%20PPGQ%20-%20UFSCar%20-%202018%20-%202%20.pdf605984d741d599e6e85a98196399e9d9MD51LICENSElicense.txtlicense.txttext/plain; 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dc.title.por.fl_str_mv |
Catalisadores a base de Pt suportados em matrizes mesoporosas de carbono visando a reação de eletrooxidação de glicerol |
dc.title.alternative.eng.fl_str_mv |
Pt-based catalysts supported in mesoporous carbon matrix for glycerol electro-oxidation reaction |
title |
Catalisadores a base de Pt suportados em matrizes mesoporosas de carbono visando a reação de eletrooxidação de glicerol |
spellingShingle |
Catalisadores a base de Pt suportados em matrizes mesoporosas de carbono visando a reação de eletrooxidação de glicerol Andrade, Renato Nunes de Células a combustíveis Eletrocatálise Glicerol Fuel cells Electrocatalysis Glycerol CMK3 CMK5 CIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA |
title_short |
Catalisadores a base de Pt suportados em matrizes mesoporosas de carbono visando a reação de eletrooxidação de glicerol |
title_full |
Catalisadores a base de Pt suportados em matrizes mesoporosas de carbono visando a reação de eletrooxidação de glicerol |
title_fullStr |
Catalisadores a base de Pt suportados em matrizes mesoporosas de carbono visando a reação de eletrooxidação de glicerol |
title_full_unstemmed |
Catalisadores a base de Pt suportados em matrizes mesoporosas de carbono visando a reação de eletrooxidação de glicerol |
title_sort |
Catalisadores a base de Pt suportados em matrizes mesoporosas de carbono visando a reação de eletrooxidação de glicerol |
author |
Andrade, Renato Nunes de |
author_facet |
Andrade, Renato Nunes de |
author_role |
author |
dc.contributor.authorlattes.por.fl_str_mv |
http://lattes.cnpq.br/9933821460129238 |
dc.contributor.author.fl_str_mv |
Andrade, Renato Nunes de |
dc.contributor.advisor1.fl_str_mv |
Sitta, Elton Fabiano |
dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/4326476348284298 |
dc.contributor.authorID.fl_str_mv |
d16278b3-dc1e-43a7-a061-b1e1c2c02959 |
contributor_str_mv |
Sitta, Elton Fabiano |
dc.subject.por.fl_str_mv |
Células a combustíveis Eletrocatálise Glicerol |
topic |
Células a combustíveis Eletrocatálise Glicerol Fuel cells Electrocatalysis Glycerol CMK3 CMK5 CIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA |
dc.subject.eng.fl_str_mv |
Fuel cells Electrocatalysis Glycerol CMK3 CMK5 |
dc.subject.cnpq.fl_str_mv |
CIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA |
description |
This work aimed the synthesis, characterization and electrochemical tests of Pt and Pt-Sb nanoparticle catalysts onto mesoporous carbon applied to glycerol electrooxidation reaction. Specifically, the carbon matrixes were synthetized from Si templates with distinct geometries, giving CMK-3 and CMK-5 3D structures. These structures were treated in O2-free atmospheres at 1173 K for 5 h and after the removal of Si with HF solution (as confirmed by thermogravimetric analysis), the mesoporous structures were attested by Small Angle X-Ray diffraction and a 4.8 and 5.3 nm porous diameters were estimated by nitrogen adsorption isotherms to the CMK-3 and CMK-5 structures, respectively. Pt nanoparticles synthesis onto carbon structures (Pt/C) were performed by direct reduction of chloroplatinic acid (H2PtCl6) with formic acid giving particles with 4.5 nm mean diameters as reveled by transmission electron microscopy. Finally, Pt-Sb/C catalysts were produced by irreversible Sb2O3 adsorption. Pt/C catalysts showed voltammetric profiles consistent with metallic Pt in 0.5 mol L-1 H2SO4 solutions, certifying the synthesis success. In the presence of glycerol, it was observed that the activity to the oxidation happens at potential higher than 0.8 V regardless the carbon support; on the other hand, Pt-Sb/C shifted the reaction onset in ca -0.3 V and maintained this activity under fixed potential (0.5 V). Pt-Sb/CMK-3 depicted the best activity among the synthetized catalysts, providing currents 1.6 and 2.0 times bigger than those in Pt-Sb/CMK-5 and Pt-Sb/Vulcan, respectively. |
publishDate |
2018 |
dc.date.issued.fl_str_mv |
2018-08-24 |
dc.date.accessioned.fl_str_mv |
2019-02-05T13:24:59Z |
dc.date.available.fl_str_mv |
2019-02-05T13:24:59Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/masterThesis |
format |
masterThesis |
status_str |
publishedVersion |
dc.identifier.citation.fl_str_mv |
ANDRADE, Renato Nunes de. Catalisadores a base de Pt suportados em matrizes mesoporosas de carbono visando a reação de eletrooxidação de glicerol. 2018. Dissertação (Mestrado em Química) – Universidade Federal de São Carlos, São Carlos, 2018. Disponível em: https://repositorio.ufscar.br/handle/ufscar/10907. |
dc.identifier.uri.fl_str_mv |
https://repositorio.ufscar.br/handle/ufscar/10907 |
identifier_str_mv |
ANDRADE, Renato Nunes de. Catalisadores a base de Pt suportados em matrizes mesoporosas de carbono visando a reação de eletrooxidação de glicerol. 2018. Dissertação (Mestrado em Química) – Universidade Federal de São Carlos, São Carlos, 2018. Disponível em: https://repositorio.ufscar.br/handle/ufscar/10907. |
url |
https://repositorio.ufscar.br/handle/ufscar/10907 |
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por |
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600 600 |
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info:eu-repo/semantics/openAccess |
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openAccess |
dc.publisher.none.fl_str_mv |
Universidade Federal de São Carlos Câmpus São Carlos |
dc.publisher.program.fl_str_mv |
Programa de Pós-Graduação em Química - PPGQ |
dc.publisher.initials.fl_str_mv |
UFSCar |
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Universidade Federal de São Carlos Câmpus São Carlos |
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Repositório Institucional da UFSCAR |
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